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Soil gas radon and thoron measurements in some

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 Author's personal copy
J Radioanal Nucl Chem
DOI 10.1007/s10967-015-4354-4

Soil gas radon and thoron measurements in some Venezuelan

oilfields
Daniel Palacios Fernández1 • Emidio Fusella2 • Yininber Avila1 • Jhonny Salas3 •
Diana Teixeira1 • Guillermo Fernández4 • Laszlo Sajo-Bohus1 • Eduardo Greaves1 •

Haydn Barros1 • Manuel Bolı́var5 • Jimmy Regalado5

Received: 22 September 2014

Ó Akadémiai Kiadó, Budapest, Hungary 2015

Abstract Radon and thoron concentrations in soil gas Macroseeps occur where gas migrate through faults or
were studied in some Venezuelan oilfields using passive fractures in the rock carrying out minor soil gases as radon.
and active methods. In some cases, investigations indicated Radon gas has been recognized as a potential tracer of fault
a strong correlation between oil production areas and the systems [1–5] because of (1) the ubiquity of its parent
intensity of radon signals, while in others a decrease in nuclides, (2) its enhanced mobility as a gas, (3) its inert
radon concentration was observed. This behavior was chemical nature, (4) its relatively short half-life, and (5) the
explained on the basis of different geological structures of high sensitivity and ease of detection. Deep origin signals
the associated reservoir traps. Geological faults associated can be observed only if convection/advection occurs, radon
with petroleum systems were well recognized by the radon being carried upward to soil surface by arising gas/water
and thoron anomalies. Possible conduits and sources column [6, 7]. This transport disturbs the radon diffusion
responsible for the occurrence of natural gas in a river and profile from the first meters of soil into the atmosphere.
in an aquifer were identified and localized. Hence the measurement of the radon concentration in soil,
at the same depth from one sampling site to the next,
Keywords Radon  Thoron  Geological fault  Natural provides a method to locate and identify the extent of zones
gas  Aquifer  Hydrocarbon exploration  LR-115 affected by advective gas mass transport. In general, radon
detectors  Lucas cells activities increase with the increase in the flow rate of the
soil-gas [6, 8, 9]. The radon/thoron ratio indicates if both
isotopes have been brought to the surface by other carrier
Introduction gases from a deeper source [10]. Since 222Rn has a much
longer half-life than 220Rn, it can be transported from
Oil and gas reservoirs often leak low molecular weight greater depths before decaying.
components of the accumulated hydrocarbons. These gases Microseeps are formed when ultrasmall (colloidal-size)
migrate toward the surface through two distinct pathways gas bubbles of light hydrocarbons migrate vertically from
that result in either prolific macroseeps or microseeps. reservoir to the surface through a water-filled network of
fractures, joints, and bedding planes by a buoyancy driven
process that results in a diffuse plume overlying the
& Daniel Palacios Fernández hydrocarbon deposit [11]. In either of the two migration
[email protected] pathways as the hydrocarbons approach the surface they
1
Universidad Simon Bolivar (USB), P.O. 89000, Caracas,
are chemically degraded and metabolized by sulfate-re-
Venezuela ducing bacteria which create a chemically reducing envi-
2
Instituto de Estudios Avanzados (IDEA), Caracas, Venezuela
ronment. Carbon dioxide and hydrogen sulfide formed by
3
bacterial and chemical hydrocarbon degradation are the
Universidad Central de Venezuela, Caracas, Venezuela
alteration agents responsible for producing, among others,
4
Universidad del Zulia, Maracaibo, Venezuela decreased potassium, and occasionally increased uranium
5
Servicios Geofı́sicos-PDVSA, Puerto la Cruz, Venezuela above many petroleum deposits [12–14]. Carbon dioxide

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forms carbonic acid in groundwater which can leach one-minute counting periods. Radon and thoron concen-
potassium and uranium from soil clays, while the chemi- trations were calculated from the recorded count rates.
cally reducing environment can concentrate uranium. Thus, Radon in soil gas by the passive method was measured
over petroleum accumulations the amount of uranium is a using LR-115 type II track detectors from Dosirad Co.,
function of dynamic equilibrium between the rate of France, fixed at the bottom of cylindrical diffusion cham-
leaching and the amount of buildup while potassium will bers (65 mm diameter and 75 mm height high-density
always decrease due to leaching. Thorium is considered to plastic cups). The top of the diffusion chambers were
be unaffected by the ascending hydrocarbons. If uranium covered with a 30 lm thick polyethylene foil to keep
reduction prevails the radon levels in pores of soils and aerosols, radon daughters and thoron gas out of the mea-
sediments over hydrocarbon reservoirs will probably be suring volume. Three cups with radon detectors inside were
lower and consequently a reduced total gamma ray flux is located at the bottom of each hole drilled at 60 cm depth.
expected. Moreover, the destruction of clay minerals by The holes were covered with the extracted soil. The time of
carbonic and organic acids also causes a higher surface exposure was 45 days. Detector etching was done under
area to volume ratio which will lead to higher efficiencies standard conditions (10 % NaOH solution at 60 °C during
of escape of 222Rn from the mineral matrix (increase of the 120 min). After etching, films were washed with distilled
emanation coefficient). For example, Matolin et al. [2] water and dried in a dust free chamber. The alpha tracks
found lowest uranium content above an oil-producing zone, recorded on the films were counted using an optical
nevertheless they noted increased levels of radon and microscope coupled to a digital camera. Track images were
thoron in that area, which they attribute to enhanced gas processed by the ImageJ free Internet access software.
emanation from U- and Th-bearing minerals decomposed Relative radon concentrations were given by the average
by hydrocarbon-generated groundwater acids (‘‘enhanced track densities since the exposure time, etching conditions
emanation power’’). and method of track reading were the same for all detec-
Several studies show that highest radon values are tors. The advanced geostatistical methods (Variogram
toward boundary of some fields, particularly those con- Analysis and Kriging) implemented in the GS? program
trolled by a regional fault [15–17]. Positive radon anoma- [23], were used for obtaining the contour maps of radon
lies at surface may be due to dissolved radium in upward and thoron concentrations in soil gas.
migrating formation water, and possibly radon carried by
upward moving gaseous hydrocarbons. Radon and other
radiometric anomalies over fault trap-type are in the form Results and discussion
of a high, and the remainder of the trap types yield a low
above the pool [18–21] or a minima confined by maximum Case study 1. Amarilis oilfield: Monagas state
values [22]. In this study three oil field sectors in eastern
Venezuela were evaluated to establish the existence of a The play Amarilis is a complex reservoir, where the exis-
correlation between zones of radon anomalies and loca- tence of several structural highs was confirmed and an
tions of active oil producing wells. The possibility to anticline fold was defined in the area drilled by the AML-
identify and localize faults or fracture systems responsible 1X well. In the AML-1X well about eight prospective
of surficial natural gas seepage will be also evaluated. intervals were identified and evaluated; only two of them
resulted oil producers (4847–4863 m and 4987–4992 m).
The only interval evaluated in the AM-2 well
Radon measurement methods and data analysis (5198–5203 m) resulted without manifestation in surface,
zero head pressure, and presence of mud and formation
Soil radon concentration was measured by active and water. The objective of this case study was to test the
passive techniques in georeferenced sites located on tran- correctness of the assumed correlation between radiometric
sects or grids. In the active measurement, soil gas was anomaly and the petroleum reservoir. The distribution of
sampled through steel sampling tubes at a depth of 60 cm. radon concentrations in soil gas along a selected transect
Radon and thoron measurements were performed with was measured to determine possible causes of differences
radiation monitors (AB-5 Pylon, Ottawa, Canada) coupled in productivity of two drilled wells. A set of 40 points for
with 270-cm3 Lucas cells. The monitors were adapted with measurements were programmed, in which each one was
a simple external filtering system to eliminate moisture and separated 250 m along a transect passing through the well
small soil particles. Flow meters were also employed to AML-1X in production and the exploratory well AML-2
ensure the cells were completely full with soil gas at the (which turned out to be dry), as given in Fig. 1.
end of the pumping cycle for thoron corrections. The The radon profile in terms of a-tracks cm-2, normalized
pumping cycle was for three minutes followed with nine for exposure time, is shown in Fig. 2. The AML-1X well is

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Fig. 1 Amarilis Oilfield (Monagas State) map, which indicates measuring points along a transect

Fig. 2 Overlapping of relative radon concentrations along the Fig. 3 Transect overlying the structural map in depth at a level close
transect with the structural map at the top of the range of interest to the producing sand discovered by the AML-1X well
(the interpreted structural folds shown)

differential compaction of the overlying sediments [22].

located along the transect with low radon concentrations Since no more maximum values in radon concentration
limited at its boundaries by the maximum values. Since an were obtained along the line farther away from the AML-2
anticline fold in the area drilled by the AML-1X well has well (in the NE direction), it must be assumed, that the well
been defined [24], this result would be consistent with the is located outside the geological dome structure and/or
mentioned model proposed by Fleisher and Turner [25], there isn’t any active fault at least until the point where the
and the suggested by Sikka and Shives [26], if the maxi- last measurement was acquired. Nevertheless, the obtained
mum had coincided with the edges of the dome. There is an results do not allow to clarify the cause why the AML-2
overlap of the obtained results with the structural map at well resulted dry.
the top of the interval of interest, therefore, it seems, that Further measurements indicated highest radon concen-
the theoretical model departs from the expected situation. trations at the oil field location of ‘‘Amarilis Oeste’’ site.
According to the model, on the edge of the dome there is an The associated geological structure, in the SW direction of
absence of cap rock and/or an increase in the number of the AML-1X well (Fig. 3), indicates that an easier gas
cracks, providing channels for the migration of gases. conduit is available for fluid transport from deeper layers
Higher radon concentration values do not lie over the through zones of enhanced permeability that, probably,
projection of possible fractures produced as a result of formed by a fault located at the south of the geological

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layer. As Sikka and Shives [22] pointed out, the possible possibly due to the complexity of the reservoir. Anyway,
causes for high radon values observed over the reservoir such radon behavior was not observed around the well that
borders are faults formed by differential compaction, turned out dry. Apparently, the productive well is located
which enhance the permeability. Accordingly, our results in an area with well-developed migration pathways and an
may be related to a geochemically active fault (indicated as active petroleum system.
GAF in Fig. 3), where gases leak out with sufficient pres-
sure to show a radon concentration anomaly. Thus, the Case study 2. Nodosaria 15, Jusepin: Monagas state
referred site can be considered as potentially hydrocarbon
bearing zone at a given depth. The productive well seems This survey was conducted in an oilfield in exploitation for
to be near the boundary of the anticlinal structure. many years where there are active and non-active wells.
Figure 4 shows the variations of the 226Ra/232Th ratios This oilfield has its northern border in the Pirital shifting
along the transect; in this case measurements were carried fault and in the western border a transversal NE fault,
out by a combination of their gamma emitting progenies which has a displacement of up to 10000 (Fig. 5). The
[26, 27]. In all cases, minimum values around the producer objective was to assess whether or not there are radon
well were obtained while nearby the dry well higher values anomalies associated with oil production sites and the type
were observed, approximately the same as in the rest of the of reservoir trap (fault trap). Most oil wells in the study
NE stations. The decrease of eU relative to thorium is in area have depths between 1900 and 2100 m. The survey
correspondence with the chemical alterations induced by consisted of 124 measurement stations distributed on a grid
the ascending hydrocarbons. Based on these results, the array of 200 m spacing.
anomaly related to a petroleum accumulation at depth, Figure 6 shows the radon and thoron contour maps
support the conclusion that the AML-1X well is located in obtained by the active method (Lucas cells). Soil pore
an area of an active petroleum system. On the other hand, radon and thoron concentration maps reflect anomalous
the dry well is located in a stretch of the transect where no high concentrations (higher than 20 and 16 kBq/m3 for
radiometric anomaly could be associated with hydrocarbon radon and thoron, respectively) overlying an area of the
seeps indicating a reservoir. fault system as indicated by the geological map. Radon and
thoron levels at the fault were higher by a factor of 2–3
Conclusions than away from the faults. Nevertheless, the distributions
are not consistent with the hypothesis that the entire fault
The productive well is characterized by a relatively low lines cross at the point with the maximum values of radon
radon concentration in soil pores compared with its sur- and thoron concentrations, possibly due to the influence of
roundings. Nevertheless, the radon profile did not spatially the environmental and climatic variations on the active
coincide with the anticlinal trap structure according to the measurements. In general, radon and thoron data show
model based on the variations of surface gas flux gradient, good correlation. The higher radon and thoron concentra-
tions were found in an area occupied by some oil wells.
Figure 7a shows the contour map for the radon/thoron
ratios obtained by the active method. The contour map
reveals anomalous high near the intersection of two faults
and, in general, radon gradient with high values to the
northeast area. Radon/thoron ratios near the intersection of
the faults were higher by a factor of 3–4 in comparison to
any other point. This result seems to indicate that gases are
transported from the greatest depth in the area where faults
intersect.
The contour map of relative radon concentrations in
soil gas obtained by passive method (LR-115 detectors in
diffusion chambers) is shown in Fig. 7b. Inspection of
the contour map reveals that detectors closest to fault
region showed alpha track density well above the back-
ground level indicating well defined radon anomaly.
Radon levels at the fault were higher by a factor of 2–4
than away from the faults. The maximum value is located
Fig. 4 Overlapping of radium normalized-thorium ratios along the in an area traversed by the fault system and near the
transect with the structural map at the top of the range of interest intersection of the two faults. Thus, the highest radon

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Fig. 5 Study area showing the locations of some oil wells and a section of the fault system associated with the oil reservoir. Measurements sites
were located at the center of the grid cells

Fig. 6 Interpolation of the radon and thoron concentrations. The overlay of the fault system and the oil well locations to the contour maps are
also shown

concentrations were found almost in all the area occupied edges of the reservoir acting as pathways for gas migration
by oil wells and at the surface along the all trace of the to the surface.
fault system.
Results indicate that radon emissions in the studied area Conclusions
are structurally controlled, which is in correspondence with
the fault trap structure of the Nodosaria-15 reservoir. The studied area shows high values of radon and thoron
Radon maximum overlies fault zones developed at the concentrations along/near the fault system as compared to

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Fig. 7 Overlap of the faults and locations of oil wells with the contour maps of the radon/thoron ratios (a) and the relative radon concentrations
obtained by the passive method (b)

the adjoining areas. Radon highs overlie the fault system the active and passive methods, soil samples were collected
regardless of the measurement method. The anomaly is in at the same measuring sites in order to determine 226Ra
correspondence with the fault trap structure of the reser- concentration. It is expected that radon concentration at
voir, so the existence of well-defined radon anomalies equilibrium can be derived to discriminate the radon
above fault-controlled oil-bearing traps was confirmed. A component rising up from a deep gas source along per-
good spatial correspondence was obtained between radon meable pathways (faults). Data were collected on a grid
anomalies and the oil wells. Measurements performed with composed of eight sets of rectangular rings centered on the
nuclear track detectors revealed with less uncertainty the locations of the two contaminated water wells, four aban-
fault system and the oil well locations for this reservoir doned gas wells suspected of gas leaks and the river
type compared to active techniques. Highs of radon relative location where gas was observed to emanate. The survey
concentrations (by the passive method) and radon/thoron consisted of 210 survey stations, 250 m apart, covering
ratio (by the active method) are spatially better correlated approximately 22 km2.
with the intersecting fault system. The results also suggest
the existence of a geochemically active fault system Active radon measurements
associated to an oil reservoir that induces radon anomaly.
The region C (Fig. 9 left) is characterized by lowest radon
Case study 3. Freites municipality: Anzoátegui state levels that indicate with high probability the presence of a
hydrocarbon reservoir in depth; this observation is sup-
The study was conducted in a locality of Freites munici- ported by laboratory gamma spectrometric results [27].
pality, Anzoátegui state, Venezuela (Fig. 8). In this region, The contour maps of soil gas 222Rn concentrations has the
two water wells resulted contaminated by natural gas and expected configuration obtained by the model based on the
gas leaks exist did show up in nearby river. They supply the alteration of near-surface gas flux gradient; in fact a locally
village located in an area where there are both active and decreased radon emanation can be identified over oil/gas
inactive oil wells, must of the last abandoned for more than reserves [25, 28]. The radon maximum concentration val-
50 years. Producing reservoir sands are at a depth between ues are near the location where gas emanates from the river
1250 and 1850 m. The objectives of this study were (1) to (zone A) (Fig. 9 left). Apparently, the anomaly located at
identify and locate possible geological faults or fractures zone A can be related to hydrocarbon gas migration
system related to methane ascension and suggest which is from a non-specified source through an interconnected
or may be the source responsible for its occurrence in the fracture system or a given fault. The radon/thoron ratios
river and aquifer, and (2) to assess whether or not there are also show an anomaly spot well defined only in
radon anomalies associated with oil production areas. In zone A (Fig. 9 right). Since both anomalies spatially co-
addition to soil in situ radon and thoron measurements by incide and as 222Rn has a much longer half-life than 220Rn,

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Fig. 8 Map of Anzoátegui state and the studied region (left). Measuring sites, contaminated water wells, gas wells suspected of gas leaks, and
location of gas emanation in the river are shown on right

222
Fig. 9 Contour maps of soil gas Rn concentrations (left) and radon/thoron ratios (right) in the studied region. Concentrations were obtained
by the active method

this result indicates that both isotopes have been brought to Passive radon measurements
the surface by associated gas carrier from a deep source
[10]. The observed river gas emanations could there- Nuclear track methodology (NTM) was followed to
fore explain the existence of an underlying hydraulic determine the relative radon concentration for the contour
connection with the aquifer and a deep fault in the map given in Fig. 10 (left). The map reports data of
referred location, being this a source of gases trans- detected track densities obtained by exposing a large set of
ported to the surface that during ascension penetrate in LR-115 type passive detectors at the selected sites. The
the aquifer. map provides the localization of a zone identified by A -
The range of values of radon concentrations shown in near the river gas emanation in that a surficial radon con-
Fig. 9 (*0.8–5.5 kBq/m3) indicates relatively low centration anomaly, i.e., where high radon concentrations
radioactivity of rocks and soil aggregates in the study area. are reported, is apparent. However, the highest radon
However, these values can be considered reliable since the concentrations were found in zone B, where there are a few
used Lucas cells have a large volume allowing radon abandoned gas wells. Such behavior can be explained by
detection with high sensitivity. According to the manu- the relatively high 226Ra (214Bi) concentrations found near
facturer the Lowest Activity Detectable for these cells is the same area as evidenced in Fig. 10-right. The homo-
27.4 Bq/m3 which is much lower than the lowest measured geneity in the geological characteristics of the study area
activity. To ensure accurate measurement results the cali- does not seem to support the assumption that 226Ra accu-
bration of the radon monitor was checked before and after mulation is related to lithological variations. This would
the field measurements. suggest that in this case, both radon and 226Ra are dragged

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Fig. 10 Contour map of the relative 222Rn concentrations in soil pores obtained by the passive method (left), and interpolation of 226
Ra
concentrations (214Bi) in surface soil samples using high resolution gamma spectrometric analysis (right)

by an upward gas flow along the pipe of one of the aban- Draws attention the differences between active and
doned wells. This explication is supported by the presence passive soil gas radon concentration measurements, par-
of gas bubbles in the area that surrounds the well-head (a ticularly in the central part of the study area. In this region
well, which has, as the technical staff suspects, gas leaks). passive method yielded radon concentrations that were
As can be seen, an apparent spatial 226Ra concentrations lower than those determined from active methods. Several
connection exists with the nearest water-well that already authors have used active and passive systems to measure
did show methane gas escape. Unlike the results given by radon in soil and radon emanation factors, and the results
active measurement method, radon levels by the passive were in general agreement with each other [29, 30].
technique seem to point toward this area (B) as possibly Ruckerbauer and Winkler [31], however, found no signif-
linked with the source that pollutes the aquifer site; since icant differences for active and passive procedures in a
soil gas radon concentrations show a steady gradient, in porous soil. Nevertheless, passive procedures yield soil
fact, its intensity gradually decreases toward the direction radon concentrations significantly lower than obtained with
where the water-wells are located. The existence of high the active procedure in an impermeable clay soil.
radon concentration and spatial connection between gas The active method indicates the radon concentration and
wells (B) and the river gas emanations (A) needs to be mobility in soil at the measurement time only. Integral
highlighted, that points toward the possible presence of a methods decrease the influence of temporal variations of the
breakdown in the structure of any of the abandoned gas measured parameter, because the response is summarized
wells in zone B and, therefore, should not be discarded in over a longer time interval. Nevertheless, according with
further analysis. Accumulated gases may have acquired Tanner [32] passive detection of radon isotopes depends on
enough pressure to migrate through a system of intercon- diffusion of radon atoms from the sites of their generation to
nected natural fractures to the geological fault or conduit the location of the detecting device. Because some radon
that intersects the aquifer. This spatial connection of high decays en route to the passive detector in soil, the radon
radon concentrations was not observed for the active concentration measured by the detector must be less than
measurements. the concentrations in those soil pores where it is undimin-
The radon activity in equilibrium with soil radium content ished by diffusion to the detector cavity. The true radon
(measured indirectly by 214Bi activity concentrations in soil concentration may be significantly underestimated espe-
samples) is very low in zone A (Fig. 10 right) compared to cially in moist soils, or when large detector cavities are
the high radon values measured in situ (Figs. 9 left and 10 used. To reduce these effects, our measurements were car-
left). This confirms the assumption of other source of radon ried out during the dry period and the used diffusion
that could originate from deep layers and migrate to the chambers were small with a semipermeable membrane
surface along a fault. Otherwise, radon values measured in covering the entrance to minimize the entry of water vapor
A had been in equilibrium with the soil radium content. and to keep aerosols, radon daughters and thoron gas out of
The lowest eU (214Bi) levels in C (Fig. 10 right) may the measuring volume.
indicate the existence of a hydrocarbon reservoir in depth, According to results of Tanner [33], for a small cavity
according to the model of radiometric anomalies over radius (B3 cm), pore water fraction less than 0.8 and
anticlinal-type hydrocarbon reservoirs. Geological data porosity about 0.4, the apparent concentration at the pas-
confirmed the previous statement and at present several oil sive detector is equal to the actual average radon concen-
wells are producing very close to that area. tration in soil gas. If the first two conditions are meet, as in

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our case, the differences between results of active and North-East of the studied area. On the other hand,
passive techniques will be greater the lower the porosity. the lowest radon concentration values detected in the
Thus, according with [31] our results seem to indicate eastern area provide information on the presence of anti-
significant differences in soil porosity in different parts of cline hydrocarbon reservoir; in fact several active wells are
the study area. operational in that area.
The fact that radon measurements by active and passive
method differ does not mean that one is better than the Acknowledgments This study has been partially financed by Rep-
sol Exploración Venezuela, S.A (LOCTI Project GPIE 33-2079/
other, or that one is correct and the other not, but rather 4916), FONACIT (Project S1-2001000954), Brazilian Agency
reflect the different behavior of the soil (by its physical FAPESP (N° 2013/13238-5) and UNIFESP.
characteristics) with respect to the way of the gas transport,
and their results are complement each other. The central
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